All-Optical Manipulation of Electron Spins in Carbon-Nanotube Quantum Dots

We demonstrate theoretically that it is possible to manipulate electron or hole spins all optically in semiconducting carbon nanotubes. The scheme that we propose is based on the spin-orbit interaction that was recently measured experimentally; we show that this interaction, together with an external magnetic field, can be used to achieve optical electron-spin state preparation with a fidelity exceeding 99%. Our results also imply that it is possible to implement coherent spin rotation and measurement using laser fields linearly polarized along the nanotube axis, as well as to convert spin qubits into time-bin photonic qubits. We expect that our findings will open up new avenues for exploring spin physics in one-dimensional systems

Molecular cavity optomechanics: a theory of plasmon-enhanced Raman scattering

The conventional explanation of plasmon-enhanced Raman scattering attributes the enhancement to the antenna effect focusing the electromagnetic field into sub-wavelength volumes. Here we introduce a new model that additionally accounts for the dynamical and coherent nature of the plasmon-molecule interaction and thereby reveals an enhancement mechanism not contemplated before: dynamical backaction amplification of molecular vibrations. We first map the problem onto the canonical model of cavity optomechanics, in which the molecular vibration and the plasmon are \textit{parametrically coupled}. The optomechanical coupling rate, from which we derive the Raman cross section, is computed from the molecules Raman activities and the plasmonic field distribution. When the plasmon decay rate is comparable or smaller than the vibrational frequency and the excitation laser is blue-detuned from the plasmon onto the vibrational sideband, the resulting delayed feedback force can lead to efficient parametric amplification of molecular vibrations. The optomechanical theory provides a quantitative framework for the calculation of enhanced cross-sections, recovers known results, and enables the design of novel systems that leverage dynamical backaction to achieve additional, mode-selective enhancement. It yields a new understanding of plasmon-enhanced Raman scattering and opens a route to molecular quantum optomechanics.Comment: Extensively revised and improved version thanks to the hard work and constructive comments of a careful Referee. Includes Supplemental Materia

Heralded single phonon preparation, storage and readout in cavity optomechanics

We analyze theoretically how to use the radiation pressure coupling between a mechanical oscillator and an optical cavity field to generate in a heralded way a single quantum of mechanical motion (a Fock state), and release on-demand the stored excitation as a single photon. Starting with the oscillator close to its ground state, a laser pumping the upper motional sideband leads to dynamical backaction amplification and to the creation of correlated photon-phonon pairs. The detection of one Stokes photon thus projects the macroscopic oscillator into a single-phonon Fock state. The non-classical nature of this mechanical state can be demonstrated by applying a readout laser on the lower sideband (i.e. optical cooling) to map the phononic state to a photonic mode, and by performing an autocorrelation measurement on the anti-Stokes photons. We discuss the relevance of our proposal for the future of cavity optomechanics as an enabling quantum technology.Comment: Accepted for publication in Physical Review Letters. Added References 42,4

Preparation and decay of a single quantum of vibration at ambient conditions

A single quantum of excitation of a mechanical oscillator is a textbook example of the principles of quantum physics. Mechanical oscillators, despite their pervasive presence in nature and modern technology, do not generically exist in an excited Fock state. In the past few years, careful isolation of GHz-frequency nano-scale oscillators has allowed experimenters to prepare such states at milli-Kelvin temperatures. These developments illustrate the tension between the basic predictions of quantum mechanics that should apply to all mechanical oscillators existing even at ambient conditions, and the complex experiments in extreme conditions required to observe those predictions. We resolve the tension by creating a single Fock state of a vibration mode of a crystal at room temperature using a technique that can be applied to any Raman-active system. After exciting a bulk diamond with a femtosecond laser pulse and detecting a Stokes-shifted photon, the 40~THz Raman-active internal vibrational mode is prepared in the Fock state $|1>$ with $98.5\%$ probability. The vibrational state is read out by a subsequent pulse, which when subjected to a Hanbury-Brown-Twiss intensity correlation measurement reveals the sub-Poisson number statistics of the vibrational mode. By controlling the delay between the two pulses we are able to witness the decay of the vibrational Fock state over its $3.9$ ps lifetime at room temperature. Our technique is agnostic to specific selection rules, and should thus be applicable to any Raman-active medium, opening a new generic approach to the experimental study of quantum effects related to vibrational degrees of freedom in molecules and solid-state systems

Photon Antibunching in the Photoluminescence Spectra of a Single Carbon Nanotube

We report the first observation of photon antibunching in the photoluminescence from single carbon nanotubes. The emergence of a fast luminescence decay component under strong optical excitation indicates that Auger processes are partially responsible for inhibiting two-photon generation. Additionally, the presence of exciton localization at low temperatures ensures that nanotubes emit photons predominantly one by one. The fact that multiphoton emission probability can be smaller than 5% suggests that carbon nanotubes could be used as a source of single photons for applications in quantum cryptography.Comment: content as publishe

An integrated source of spectrally filtered correlated photons for large scale quantum photonic systems

We demonstrate the generation of quantum-correlated photon-pairs combined with the spectral filtering of the pump field by more than 95dB using Bragg reflectors and electrically tunable ring resonators. Moreover, we perform demultiplexing and routing of signal and idler photons after transferring them via a fiber to a second identical chip. Non-classical two-photon temporal correlations with a coincidence-to-accidental ratio of 50 are measured without further off-chip filtering. Our system, fabricated with high yield and reproducibility in a CMOS process, paves the way toward truly large-scale quantum photonic circuits by allowing sources and detectors of single photons to be integrated on the same chip.Comment: 4 figure

Nonlinear characterisation of a silicon integrated Bragg waveguide filter

Bragg waveguides are promising optical filters for pump suppression in spontaneous Four-Wave Mixing (FWM) photon sources. In this work, we investigate the generation of unwanted photon pairs in the filter itself. We do this by taking advantage of the relation between spontaneous and classical FWM, which allows for the precise characterisation of the nonlinear response of the device. The pair generation rate estimated from the classical measurement is compared with the theoretical value calculated by means of a full quantum model of the filter, which also allows to investigate the spectral properties of the generated pairs. We find a good agreement between theory and experiment, confirming that stimulated FWM is a valuable approach to characterise the nonlinear response of an integrated filter, and that the pairs generated in a Bragg waveguide are not a serious issue for the operation of a fully integrated nonclassical source

Energy correlations of photon pairs generated by a silicon microring resonator probed by Stimulated Four Wave Mixing

Compact silicon integrated devices, such as micro-ring resonators, have recently been demonstrated as efficient sources of quantum correlated photon pairs. The mass production of integrated devices demands the implementation of fast and reliable techniques to monitor the device performances. In the case of time-energy correlations, this is particularly challenging, as it requires high spectral resolution that is not currently achievable in coincidence measurements. Here we reconstruct the joint spectral density of photons pairs generated by spontaneous four-wave mixing in a silicon ring resonator by studying the corresponding stimulated process, namely stimulated four wave mixing. We show that this approach, featuring high spectral resolution and short measurement times, allows one to discriminate between nearly-uncorrelated and highly-correlated photon pairs.Comment: 7 pages, 4 figure